Although ZIF-based adsorbents are promising for environmental remediation, their performance is limited by their large crystal size, intrinsic fragility, and poor processability and reusability. To this end, in this work, highly dispersed and small sized (14.95 nm) metal−organic frameworks (MOFs), via the restriction of overgrowth and agglomeration on carbon nitride (C 3 N 4 ) nanosheets, are integrated into agar aerogel, forming a flexible and efficient aerogel absorbent with photocatalytic activity. This separationfree hybrid aerogel mantaining the crystal structure of zeolitic imidazolate framework (ZIF-8) with smaller size exhibits a 1.44 times greater adsorption capacity for dye than that of pristine bulk ZIF-8. Most importantly, the introduction of C 3 N 4 nanosheets not only regulates the growth of ZIF-8 crystals but also enables the hybdrid aerogel with stable reusability throughout five consecutive adsorption−degradation cycles, obtained via solar irradiation. This ecofriendly, regeneration technology provides a convenient and sustainable approach to reduce the cost and eliminate the use of hazardous substances for environmental remediation. Dramatically, for practical use under sunlight, attributed to the photocatalysis effect of the uniquely designed adsorbent, the active adsorption sites of the aerogel are continuously provided, resulting in enhanced dye removal ability. Therefore, this work establishes an innovative, low-cost, convenient, solar-triggered, sustainable solution for the management of water contamination by a MOF-based aerogel decontaminant.